Regarding consular jurisdiction in Massachusetts, the split between New Bedford and Boston is especially tricky. New Bedford serves certain counties and cities in Mass., but the rest of the state (and the rest of New England) go through the Boston consulate.
The Portuguese consulates in the northeastern states from Delaware through Maine are a bit complicated when it comes to their consular jurisdiction. I thought the Portuguese embassy provided a list of these until recently, but I can't seem to find it on their website as of today. I just posted a third-party link above.
In addition, Delaware, New Jersey, and Pennsylvania are served by the Newark consulate. Rhode Island has its own special consulate.
It may be best first to check with the appropriate consulate in your consular jurisdiction before proceeding with a visa application. Consular jurisdiction may be different for visas versus for other consular activities. For all I know, some consulates may redirect visa applications to another consulate if not covered by VFS.
Aside from the above, I think all the other states, commonwealths, and territories go through VFS in one of their three US-based application centers. The jurisdiction of the New York consulate covers Connecticut, New York, and also Michigan somehow, and those states thereby can go through the application center at VFS New York.